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- W4384824972 abstract "<strong class=journal-contentHeaderColor>Abstract.</strong> Acylperoxy radicals (RO<sub>2</sub>) are key intermediates in atmospheric oxidation of organic compounds and different from the general alkyl RO<sub>2</sub> radicals in reactivity. However, direct probing of the molecular identities and chemistry of acyl RO<sub>2</sub> remains quite limited. Here, we report a combined experimental and kinetic modelling study of the composition and formation mechanisms of acyl RO<sub>2</sub>, as well as their contributions to the formation of highly oxygenated organic molecules (HOMs) during ozonolysis of α-pinene. We find that acyl RO<sub>2</sub> radicals account for 67 %, 94 %, and 32 % of the highly oxygenated C<sub>7</sub>, C<sub>8</sub>, and C<sub>9</sub> RO<sub>2</sub>, respectively, but only a few percent of C<sub>10</sub> RO<sub>2</sub>. The formation pathway of acyl RO<sub>2</sub> species depends on their oxygenation level. The highly oxygenated acyl RO<sub>2</sub> (oxygen atom number ≥ 6) are mainly formed by the intramolecular aldehydic H-shift (i.e., autoxidation) of RO<sub>2</sub>, while the less oxygenated acyl RO<sub>2</sub> (oxygen atom number < 6) are basically derived from the C-C bond cleavage of alkoxy (RO) radicals containing an α-ketone group or the intramolecular H-shift of RO containing an aldehyde group. The acyl RO<sub>2</sub>-involved reactions explain 50–90 % of C<sub>7</sub> and C<sub>8</sub> closed-shell HOMs and 14 % of C<sub>10</sub> HOMs, respectively. For C<sub>9</sub> HOMs, this contribution can be up to 30 %–60 %. In addition, acyl RO<sub>2</sub> contribute to 50 %–95 % of C<sub>14–</sub>C<sub>18</sub> HOM dimer formation. Because of the generally fast reaction kinetics of acyl RO<sub>2</sub>, the acyl RO<sub>2</sub> + alkyl RO<sub>2</sub> reactions seem to outcompete the alkyl RO<sub>2</sub> + alkyl RO<sub>2</sub> pathways, thereby affecting the fate of alkyl RO<sub>2</sub> and HOM formation. Our study sheds lights on the detailed formation pathways of the monoterpene-derived acyl RO<sub>2</sub> and their contributions to HOM formation, which will help to understand the oxidation chemistry of monoterpenes and sources of low-volatility organic compounds capable of driving particle formation and growth in the atmosphere." @default.
- W4384824972 created "2023-07-21" @default.
- W4384824972 date "2023-07-19" @default.
- W4384824972 modified "2023-10-03" @default.
- W4384824972 title "Comment on egusphere-2023-838" @default.
- W4384824972 doi "https://doi.org/10.5194/egusphere-2023-838-rc2" @default.
- W4384824972 hasPublicationYear "2023" @default.
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